Article(id=1319726291717304448, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319726202550600683, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20240809, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1734537600000, receivedDateStr=2024-12-19, revisedDate=1739808000000, revisedDateStr=2025-02-18, acceptedDate=null, acceptedDateStr=null, onlineDate=1792576867274, onlineDateStr=2026-10-21, pubDate=1755619200000, pubDateStr=2025-08-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1792576867274, onlineIssueDateStr=2026-10-21, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1792576867274, creator=13701087609, updateTime=1792576867274, updator=13701087609, issue=Issue{id=1319726202550600683, tenantId=1146029695717560320, journalId=1263187385517883426, year='2025', volume='53', issue='8', pageStart='2079', pageEnd='2418', issueExtLink='null', onlineDate='null', pubDate='1755619200000', pubDateStr='2025-08-20', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1792576846015, creator='13701087609', updateTime=1792577372688, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1319728411619213318, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319726202550600683, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1319728411619213319, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319726202550600683, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=2229, endPage=2238, ext={EN=ArticleExt(id=1319726292065431681, articleId=1319726291717304448, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Oxidation Degradation of Formaldehyde over Goethite Calcinated Product and Hexagonal Birnessite Composite at Ambient Temperature, columnId=1319726165087077079, journalTitle=Journal of the Chinese Ceramic Society, columnName=Research Article, runingTitle=null, highlight=null, articleAbstract=
Introduction Birnessite has exhibited moderate activity in room-temperature oxidation degradation of formaldehyde and is considered as the most promising material for formaldehyde degradation. However, birnessite also exposed insufficient surface active sites to meet the needs for long-term and sufficient degradation of formaldehyde. As a cheap and easily obtainable mineral, goethite not only has a large specific surface area and high oxidation-reduction activity, but also usually appears as nanoscale particles. Hematite can be prepared via calcination of goethite, which can maintain the original needle like structure of goethite, and has a larger specific surface area than that of goethite. It is speculated that using hematite obtained by heat treatment of goethite to support hexagonal birnessite might increase the surface active sites of the catalyst, thereby improving the formaldehyde degradation activity at room temperature. Therefore, in this study, goethite was used as a precursor to prepare hematite with different specific surface areas by calcining method at different temperatures. The structure and physicochemical properties of the catalyst, the activity and mechanism of the catalyst for the oxidation and degradation of low concentration formaldehyde at room temperature were studied.
Method The synthesis method of K0.6hbir was as follows: Dissolve KMnO4 (4.00 g), MnCl2 (8.35 g), and NaOH (2.88 g) in 130, 130 mL, and 140 mL of deionized water, respectively. Firstly, slowly added KMnO4 solution to (within 5 min) NaOH solution and stirred for 1 h. After that, MnCl2 solution was added into the above mixture within 35 min and stirred for 2 h, and then aged for 4 h. After wash and centrifuge for 3 times, the generated precipitate was dried at 70 ℃. The synthesis method of hematite and birnessite composite was as follows: Goethite was calcined in a muffle furnace at 200, 250, 300, 400 ℃, and 500 ℃ for 2 h, respectively. The obtained hematite was named as Hem-X, where X represents the calcination temperature. Add the above sample to 140 mL of NaOH solution (0.18 mol/L) and stir vigorously for 30 min. Then, synthesize hematite composite birnessite sample using the method of preparing birnessite. The amount of birnessite in the composite was 30% (mass fraction), and the sample was named as K0.6hbir@Hem-X. The phase and structure of the catalyst was characterized using X-ray diffractometer (XRD, Dandong Haoyuan, DX-2700), Raman spectrometer (RAMAN, LabRAM HR Evolution), high-resolution transmission electron microscopy (TEM, JEM-2100F), respectively. The specific surface area was measured using a BET adsorption desorption instrument (BET, NOVA 3000e). Surface elemental valence states of the sample was characterized by X-ray fluorescence spectroscopy (XPS, ESCALAB250Xi). The in-situ degradation process of formaldehyde was carried out in a Fourier transform infrared spectrometer (FTIR, VERTEX 70, Bruker). The dynamic experiment for catalytic oxidation of formaldehyde was carried out in a quartz tube. 1 mg/L formaldehyde gas can be stably obtained by volatilization of polyformaldehyde under constant temperature and circulating cooling water conditions at 10 ℃. The total gas flow rate was 1 L/min corresponding to a WHSV of 1200 L/(g·h). The formaldehyde concentration before and after the reaction were detected online by a formaldehyde detector (Interscan 4160-19.99 m). CO2 was detected by gas chromatography (GC-2020) under the formaldehyde concentration of 10 mg/L.
Results and discussion Hematite obtained by calcining goethite at 300 ℃ shows a higher formaldehyde removal rate which can maintain a formaldehyde removal rate at about 90% within 2 h, as compared with the other hematite samples and goethite. Based on the results of specific surface area, the formaldehyde removal ability of hematite was closely related to its specific surface area. The K0.6hbir@Hem catalysts also exhibited the same trend as that of the bulk hematite, and had superior removal performance than hematite. K0.6hbir@Hem-300 had the best catalytic activity and maintained a removal rate of over 95% for formaldehyde within 300 min. In particular, the K0.6hbir@Hem-300 catalyst can maintain almost 100% formaldehyde removal rate in 24 h when the WHSV was 400 L/(g·h), but showed a significant decrease with the increasing of WHSV. The results of in-situ DRFITS and quenching experiments indicated that the 'O2- species promoted the transformation of DOM into formate, while the ·OH species had the effect on the completely conversion of the intermediates to CO2 and H2O during the oxidation degradation of formaldehyde.
Conclusions K0.6hbir@Hem-300 had superior formaldehyde oxidation degradation performance, achieving almost 100% formaldehyde (1 mg/L) removal rate within 24 h at 400 L/(g·h) WHSV with no activity loss over 5 cycles. The relative humidity significantly affected the oxidation degradation performance of the composite. The hematite and hexagonal birnessite composite had higher CO2 yield (55%) than that of the goethite and hexagonal birnessite composite (40%), indicating that the obtained hematite was a more suitable support than the original goethite. The specific surface area of K0.6hbir@Hem-300 (116.5 m2/g) further increased compared with that of Hem-300 (86.7 m2/g), which was beneficial to the adsorption of formaldehyde during the degradation processes. The introduction of hematite increased the contents of Mn (III) and surface active oxygen species over the composite, leading to the enhancement of oxidation degradation performance of formaldehyde. In particular, the ·O2- species promoted the transformation of DOM into formate, while the ·OH species had the effect on the completely conversion of the intermediates to CO2 and H2O during the oxidation degradation of formaldehyde.
, authors=Xuehua ZOU, Aidi HUANG, Zhengyan HAN, Jinyong CHEN, Zhilin ZHOU, Qimengzi WANG, Lingna QIAN, Haibo LIU, Tianhu CHEN, authorsList=Xuehua ZOU, Aidi HUANG, Zhengyan HAN, Jinyong CHEN, Zhilin ZHOU, Qimengzi WANG, Lingna QIAN, Haibo LIU, Tianhu CHEN, authorCompany=null, correspAuthors=Tianhu CHEN, authorNote=
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水钠锰矿具有良好的常温氧化降解甲醛活性，但单一水钠锰矿也暴露出表面活性位点不足，无法满足长期高效净化甲醛的需求。以不同温度煅烧针铁矿得到赤铁矿产物为载体，通过氧化还原法制备了系列赤铁矿复合六方水钠锰矿催化剂，探究了其在室温下氧化降解甲醛的性能及作用机制。采用X射线衍射仪、比表面积分析仪、X射线光电子能谱仪、拉曼光谱仪、透射电子显微镜和原位红外光谱仪等方法对样品进行表征。结果表明：对比赤铁矿和单一六方水钠锰矿，300 ℃煅烧针铁矿得到的赤铁矿复合水钠锰矿样品（K0.6hbir@Hem-300）室温下具有更优异的氧化降解甲醛活性，在甲醛初始浓度1 mg/L、空速为400 L/（g·h）和室温条件下，甲醛去除率在24 h内可维持在100%，且具有良好的循环稳定性。这是因为赤铁矿的引入增加了复合催化剂Mn（Ⅲ）和表面活性氧物种含量，提升了其催化氧化甲醛的能力。相较于六方水钠锰矿复合针铁矿材料，六方水钠锰矿复合赤铁矿对甲醛（10 mg/L）的氧化能力显著增强，CO2转化率约为55%，显著优于前者的40%，表明煅烧针铁矿得到的赤铁矿比原样更适合作为载体。原位红外及淬灭实验表明，在氧化降解甲醛过程中，·O2-促进DOM向甲酸盐的转化，而·OH影响中间产物向终产物CO2和H2O矿化。
, authors=邹雪华, 黄爱娣, 韩正严, 陈进永, 周之琳, 王祁梦子, 钱玲娜, 刘海波, 陈天虎, authorsList=邹雪华, 黄爱娣, 韩正严, 陈进永, 周之琳, 王祁梦子, 钱玲娜, 刘海波, 陈天虎, authorCompany=null, correspAuthors=陈天虎, authorNote=
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陈天虎（1962—），男，博士，教授。
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ZOU Xuehua (1988-), male, Ph.D., Lecturer. E-mail: zouxuehua1988@hfut.edu.cn
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邹雪华（1988—），男，博士，讲师。
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